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Title: The Nature of Electrochemical Delithiation of Li-Mg Alloy Electrodes: Neutron Computed Tomography and Modeling of Li Diffusion and Delithiation Phenomenon

Journal Article · · Journal of the Electrochemical Society
DOI:https://doi.org/10.1149/2.0051702jes· OSTI ID:1393861
 [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [3]
  1. Univ. of Utah, Salt Lake City, UT (United States). Dept. of Metallurgical Engineering
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical and Engineering Materials Division
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Data Analysis and Visualization Division
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Li-Mg alloys are promising as positive electrodes (anodes) for Li-ion batteries due to the high Li storage capacity and the relatively lower volume change during the lithiation/delithiation process. They also present a unique opportunity to image the Li distribution through the electrode thickness at various delithiation states. In this work, spatial distributions of Li in electrochemically delithiated Li-Mg alloy electrodes have been quantitatively determined using neutron tomography. Specifically, the Li concentration profiles along thickness direction are determined. A rigorous analytical model to quantify the diffusion-controlled delithiation, accompanied by phase transition and boundary movement, has also been developed to explain the delithiation mechanism. The analytical modeling scheme successfully predicted the Li concentration profiles which agreed well with the experimental data. It is demonstrated that during discharge Li is removed by diffusion through the solid solution Li-Mg phases and this proceeds with β→α phase transition and the associated phase boundary movement through the thickness of the electrode. This is also accompanied by electrode thinning due to the change in molar volume during delithiation. In conclusion, following the approaches developed here, one can develop a rigorous and quantitative understanding of electrochemical delithiation in electrodes of electrochemical cells, similar to that in the present Li-Mg electrodes.

Research Organization:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1393861
Journal Information:
Journal of the Electrochemical Society, Vol. 164, Issue 2; ISSN 0013-4651
Publisher:
The Electrochemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 17 works
Citation information provided by
Web of Science

References (18)

Water calibration measurements for neutron radiography: Application to water content quantification in porous media
  • Kang, M.; Bilheux, H. Z.; Voisin, S.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 708 https://doi.org/10.1016/j.nima.2012.12.112
journal April 2013
Neutron scattering lengths and cross sections journal January 1992
In Situ Neutron Imaging Of Alkaline and Lithium Batteries conference January 2010
Lithium insertion/extraction mechanism in alloy anodes for lithium-ion batteries journal February 2011
Anomalous Discharge Product Distribution in Lithium-Air Cathodes journal April 2012
Neutron imaging of a commercial Li-ion battery during discharge: Application of monochromatic imaging and polychromatic dynamic tomography
  • Butler, Leslie G.; Schillinger, Burkhard; Ham, Kyungmin
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 651, Issue 1 https://doi.org/10.1016/j.nima.2011.03.023
journal September 2011
Refraction contrast imaging and edge effects in neutron radiography journal February 2012
Electrochemical properties of Li–Mg alloy electrodes for lithium batteries journal January 2001
Edge Enhancement in Cold Neutron Imaging: A Comparison of Experiments at Edges and Interfaces with Ray-tracing based on Refraction and Reflection journal January 2013
Analytical modeling and simulation of electrochemical charge/discharge behavior of Si thin film negative electrodes in Li-ion cells journal February 2014
Octopus, a fast and user-friendly tomographic reconstruction package developed in LabView® journal June 2004
Lithium-rich Li2.6BMg0.05 alloy as an alternative anode to metallic lithium for rechargeable lithium batteries journal October 2011
NIH Image to ImageJ: 25 years of image analysis journal June 2012
Neutron imaging of lithium concentration in battery pouch cells conference June 2011
Fiji: an open-source platform for biological-image analysis journal June 2012
Data processing and image reconstruction methods for pixel detectors
  • Jakubek, Jan
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 576, Issue 1, p. 223-234 https://doi.org/10.1016/j.nima.2007.01.157
journal June 2007
Electrochemical Charge/Discharge Behavior and Phase Transitions during Cell Cycling of Li(Mg) Alloy Anodes for High Capacity Li Ion Batteries journal January 2013
The Li-Mg (Lithium-Magnesium) system journal August 1984

Cited By (4)

Lithium–Magnesium Alloy as a Stable Anode for Lithium–Sulfur Battery journal February 2019
Diffusion Limitation of Lithium Metal and Li–Mg Alloy Anodes on LLZO Type Solid Electrolytes as a Function of Temperature and Pressure journal October 2019
The Challenge of Lithium Metal Anodes for Practical Applications journal April 2019
ImagingReso: A Tool for Neutron Resonance Imaging journal November 2017

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36 MATERIALS SCIENCE
25 ENERGY STORAGE
Analytical model
Diffusion
Li-Mg alloy
Lithium-ion batteries
Neutron tomography